WO2002072253A1 - Empilement de substrats pour reacteurs monolithes - Google Patents
Empilement de substrats pour reacteurs monolithes Download PDFInfo
- Publication number
- WO2002072253A1 WO2002072253A1 PCT/US2002/006725 US0206725W WO02072253A1 WO 2002072253 A1 WO2002072253 A1 WO 2002072253A1 US 0206725 W US0206725 W US 0206725W WO 02072253 A1 WO02072253 A1 WO 02072253A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- reactor
- monoliths
- monolith
- substrates
- stack
- Prior art date
Links
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/32—Packing elements in the form of grids or built-up elements for forming a unit or module inside the apparatus for mass or heat transfer
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/24—Stationary reactors without moving elements inside
- B01J19/248—Reactors comprising multiple separated flow channels
- B01J19/2485—Monolithic reactors
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/32—Packing elements in the form of grids or built-up elements for forming a unit or module inside the apparatus for mass or heat transfer
- B01J19/325—Attachment devices therefor, e.g. hooks, consoles, brackets
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
- B01J2219/322—Basic shape of the elements
- B01J2219/32203—Sheets
- B01J2219/32265—Sheets characterised by the orientation of blocks of sheets
- B01J2219/32272—Sheets characterised by the orientation of blocks of sheets relating to blocks in superimposed layers
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
- B01J2219/322—Basic shape of the elements
- B01J2219/32296—Honeycombs
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
- B01J2219/324—Composition or microstructure of the elements
- B01J2219/32408—Metal
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
- B01J2219/324—Composition or microstructure of the elements
- B01J2219/32425—Ceramic
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
- B01J2219/324—Composition or microstructure of the elements
- B01J2219/32466—Composition or microstructure of the elements comprising catalytically active material
Definitions
- This invention relates to improvements in monolith reactors widely used in the chemical and refining industries, and more particularly to methods and structures for packaging, sealing and assembling large diameter substrates for monolith reactors.
- extruded honeycomb monoliths can be catalytically active or coated with a wash coating and catalyzed with an active material.
- present extrusion manufacturing limitations prevent the production of large monoliths, it is necessary to assemble a plurality of smaller monoliths such as by cementing the parts together in order to fabricate large monolithic structural shapes.
- honeycomb ceramic substrates being brittle, are subject to damage and deterioration from both expansion and vibration, and the present invention provides unique support structures to compensate for and alleviate such problems.
- U.S. Patent No. 5,108,716 discloses a catalytic converter for an automobile having a first and second monolith in a row.
- U.S. Patent No. 4,195,064 discloses a bed-type catalytic reactor having horizontal beams mounted for movement relative to vertical columns.
- European Patent Specification 0226306B 1 discloses a complex arrangement of ledges and projections that function to support and interlock adjacent ceramic structures used as catalyst supports.
- the invention describes various designs for assembling, supporting and packing monoliths within a reactor.
- a plurality of commercially available ceramic honeycomb monolithic substrates is cemented together about their outer edges, with the longitudinal axes of the adjacent honeycomb channels being parallel.
- subassemblies of such cemented substrates may be further cemented together to form larger monolith assemblies.
- the assemblies of monoliths are then stacked within a reactor housing and supported with necessary sealing under compression to avoid the deleterious effects of vibration and expansion.
- a grid- ork having a pattern similar to that of the juncture of the cemented outer edges of the monoliths may be positioned at each end of the stack of assemblies, and spring-loaded means is urged against at least one such grid-work to provide a substantially constant pressure on the stack of monoliths.
- the monoliths may be composed of metals, or of composite materials comprising mixtures of metals and ceramics, as well as ceramic materials such as zeolite, cordierite, alumina, mullite, silica or the like.
- Monoliths comprising carbon, or coatings or dispersions of carbon, may also be useful.
- Fig. 1 is schematic view in elevation, partially in section, of a reactor tank showing one embodiment for supporting a stack of monolith assemblies under compression within the tank.
- Fig. 2 A is an enlarged view of the circled area "A" of Fig. 1, showing a means for providing a compressive force to the stacked monolithic assemblies.
- Fig. 3 is an enlarged plan view of the substrate layout within the reactor of
- Fig. 1 is an enlarged plan view showing the support grid-work and pressure grid-work layout utilized at end portions of the stacked assembly of Fig. 1
- Fig. 5 is a more enlarged plan view of the ceramic substrate layout of a further embodiment of the invention showing the position of spacer members.
- Fig. 6 is a perspective view of a spacer member utilized with the layout of Fig. 5.
- Fig. 7 is a schematic view in elevation, partially in section, of a reactor tank showing another embodiment for supporting a stack of monolith assemblies under compression within the tank.
- Fig. 8B is an enlarged view of the circled area "B" of Fig. 7, showing another means for providing a compressive force to the stacked monolithic assemblies.
- Fig. 9 is an enlarged plan view of the substrate layout within the reactor of Fig. 7.
- Fig. 10 is an enlarged plan view showing the support pressure grid-work layout utilized at the upper end portion of the stacked assembly of Fig. 7.
- Fig. 1 1 is a plan view of a further embodiment showing an arrangement of a plurality of individual containers having stacked monoliths therein positioned within a reactor housing.
- a reactor housing or tank 10 having a plurality of ceramic honeycomb monoliths or substrates 12 positioned therein with the longitudinal axes of the honeycomb channels extending along parallel to the longitudinal axis a of the reactor 10.
- the monoliths 12 may be extruded in any desired shape, but for the embodiment shown, they are preferably extruded in a square shape, and four such squares are cemented together along their side edges to form a subassembly 14. Four of the subassemblies are then cemented together along edge portions to form the final assembly 16.
- the cements may be either inorganic or organic in composition, and can be cold set at room temperature or heat-treated.
- the outer monoliths 18 are cut or machined into a rounded curvature to fit within the round reactor 10. Suitable cement, such as epoxy or phenol resins mixed with any ceramic filler and a mineral binder, is then applied to the outer cut surface of the monolith assembly 16 to form a skin and provide strength and protection to the assembly.
- the reactor housing 10 includes a bottom cap 20 secured to the main housing by bolted together flanges 22a and 22b and an upper cap 24 secured to the main housing by bolted together flanges 26a and 26b.
- the caps 20 and 24 are provided with suitable inlet and outlet connections, not shown, for the flow of reactants through the reactor.
- a static mixer 28 is shown positioned in the lower cap 20 to mix incoming flows before entering the stack of honeycomb monolithic assemblies 16 within the reactor housing
- a lower suspension ring 30 is held in a clamped relationship between bolted flanges 22a and 22 b.
- the suspension ring 30 retains a support grating 32, which has a grid-work pattern similar to the cemented junctures 15 of the monoliths 12.
- a plurality of the final assemblies 16 is stacked on the support grating 32 within the reactor housing 10.
- a gasket not shown, of suitable material such as stainless steel,
- Teflon, graphite or Gortex is positioned between the support grating 32 and the bottom assembly 16 for sealing the junctions 15 of the bottom monolith assembly and with a peripheral portion for providing sealing between the inner surface of the reactor housing 10 and the outer surface of the bottom monolith assembly 16.
- Each layer of monolith assemblies 16 may be rotated up to 90 degrees or more about its longitudinal axis with respect to an adjacent assembly, or the honeycomb channel openings of adjacent monoliths may be offset from one another, so as to provide a zigzag flow path through the reactor if desired. The rotation provides a self-seal between adjacent surfaces of the stacked monolith assemblies. However, additional sealing material is provided between the monolith assemblies and the inner wall of the reactor so as to squeeze the monoliths closer together and prevent by-pass.
- a sealing gasket not shown, having a pattern similar to the junctures 15 of the individual cemented monoliths, is positioned on top of the upper monolith assembly 16 for sealing such junctures.
- a top grating or pressure grid 34 having a circular rim portion 36 adjacent the inner wall of the reactor 10, and a grid-work similar to junctures 15 between the cemented monoliths, is positioned over the sealing gasket.
- An upper suspension ring 38 having a downward circular portion 40 adjacent an inner wall portion of reactor 10, has a flange portion retained between flanges 26a and 26b.
- the upper suspension ring 38 has a plurality of radially-inwardly projecting bosses 42.
- Each boss 42 has a Belville spring washer 44 secured thereto by means of a nut member 46 affixed to the suspension ring 38.
- a lower spring-loaded portion 48 of the washer 44 engages cross members of the pressure grid 34, and applies a desired pressure thereto by means of adjustment nut 50.
- the spring-loaded washer contact with the grid 34 is shown along individual cross members, preferably such contact is at junctures of the cross members.
- the spring-loaded washers 44 provide a pressure system for the monolith assemblies 16 stacked within the reactor housing 10 to hold such assemblies together in a tight relationship and prevent deleterious vibration of the units. The pressure system also compensates for different expansions between the monolith assemblies and the reactor body.
- FIG. 5 and 6 The embodiment shown in Figs. 5 and 6 is similar to the embodiment shown in Figs. 1-4, except for the stacking of the substrate assemblies 16.
- a section of a cross spacer 52 is shown in Fig. 6.
- the spacer material may be either organic or inorganic, and may include such materials as stainless steel, Teflon, graphite and gortex.
- the vertical sections of the cross spacers 52 embed themselves in the upper and lower monolith assemblies, as they are stacked in the reactor, and with the horizontal section of the spacers function to seal the junctures of adjacent lateral monoliths.
- the cross spacers could be provided as a one-piece grid-like unit if desired.
- the packing, sealing and compression are the same as in the embodiment of Figs. 1-4.
- the embodiments of Figs. 1-6 are usually utilized in a vertical position as shown, however they may be utilized in a horizontal position.
- a further embodiment of the invention is shown in Figs. 7, 8B, 9 and 10, wherein rods 54 are utilized to support the stacked assemblies 16.
- holes 56 are formed in each of the individual monoliths 12 of the assemblies 16.
- the reactor housing is similar to that shown in Fig.
- the static mixer 28 is shown positioned within the main housing 10 on a suspension ring 30.
- the flow is preferably from the bottom to the top and may use counter flow or co-current flow as described before.
- the rods 54 go through the holes 56 in the monoliths 12 forming the assemblies 16, and the stacks are supported from the top of the reactor as shown in Fig. 8B.
- Each rod 54 has a washer or small plate 55 attached thereto to retain the monolith assemblies on the rods, and accordingly a lower support grating is not required.
- a sealing gasket and a pressure grid are positioned on top of the upper monolith assembly as before.
- the pressure grid 58 is provided with openings at the intersection of the grid members, and it is orientated so that the holes in the intersections of the grid members lie over and receive the rods 54 there through.
- a suspension ring 38 is retained between flanges 26a and 26b and retains a support grating 60.
- the upper end of the rods 54 which are threaded, extend up through the support grating 60 and are fixedly secured thereto by nuts 62, 64.
- Suitable compression means are positioned about the rods 54 such as a Belville spring washer, or a compression spring 66 urged against pressure grid 58 by an adjustment nut 68.
- the spring loading prevents vibration and pressure and temperature effects on the stacked monolith assemblies 16 by keeping them under a constant predetermined compression.
- Fig. 1 1 relates to a series of individually housed monoliths packaged together to form a large diameter assembly.
- a plurality of smaller housings 70, each containing a stack 72 of either single monoliths or of assembled monoliths is positioned within a larger housing 74.
- Each individual housing 70 may be stacked in layers to fill a reactor of any length. Again, each housing 70 is spring loaded in either manner previously described to compensate for expansion and vibration.
- Each reactor housing 70 may be provided with its own liquid distributor and gas delivery system. Although the system has more void volume compared to the previous embodiments, it provides a capability to build larger monolith assemblies with built-in support rods, with each rod being independently supported on a frame in the reactor.
Abstract
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US09/804,944 | 2001-03-13 | ||
US09/804,944 US7182924B2 (en) | 2001-03-13 | 2001-03-13 | Substrate packing for monolith reactors |
Publications (1)
Publication Number | Publication Date |
---|---|
WO2002072253A1 true WO2002072253A1 (fr) | 2002-09-19 |
Family
ID=25190284
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/US2002/006725 WO2002072253A1 (fr) | 2001-03-13 | 2002-03-05 | Empilement de substrats pour reacteurs monolithes |
Country Status (2)
Country | Link |
---|---|
US (1) | US7182924B2 (fr) |
WO (1) | WO2002072253A1 (fr) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP3785795A4 (fr) * | 2018-07-13 | 2021-05-12 | Mitsubishi Heavy Industries Engineering, Ltd. | Réacteur catalytique |
Families Citing this family (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US7109378B2 (en) * | 2001-08-30 | 2006-09-19 | Air Products And Chemicals, Inc. | Monolith catalytic reactor coupled to static mixer |
CN1312033C (zh) * | 2005-07-01 | 2007-04-25 | 清华大学 | 一种大批量制备超长碳纳米管阵列的方法 |
US8007731B2 (en) * | 2007-08-10 | 2011-08-30 | Corning Incorporated | Fluid treatment device having a multiple ceramic honeycomb layered structure |
US8697015B2 (en) | 2011-12-01 | 2014-04-15 | Chevron U.S.A. Inc. | Flow distribution for monolithic reactors |
CN105413595B (zh) * | 2015-12-24 | 2018-04-17 | 天津大学 | 带弹簧限位装置的填料压圈 |
US20210220813A1 (en) * | 2020-01-16 | 2021-07-22 | Johnson Matthey Public Limited Company | Pallet for supporting a catalyst monolith during coating |
Citations (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4195064A (en) * | 1978-08-15 | 1980-03-25 | Monsanto Company | Unitized catalytic reactor construction |
US4743578A (en) * | 1985-11-13 | 1988-05-10 | Imperial Chemical Industries Plc | Ceramic structures |
US5108716A (en) * | 1987-06-30 | 1992-04-28 | Nissan Motor Company, Inc. | Catalytic converter |
US5527631A (en) * | 1994-02-18 | 1996-06-18 | Westinghouse Electric Corporation | Hydrocarbon reforming catalyst material and configuration of the same |
WO1996033017A1 (fr) * | 1995-04-19 | 1996-10-24 | Technische Universiteit Delft | Procede de fabrication d'empilements de catalyseurs |
US6019951A (en) * | 1992-11-04 | 2000-02-01 | Technische Universiteit Delft | Catalytic reactor |
Family Cites Families (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4407785A (en) * | 1972-11-28 | 1983-10-04 | Engelhard Corporation | Method of conducting catalytically promoted gas-phase reactions |
US4323614A (en) * | 1976-03-31 | 1982-04-06 | Corning Glass Works | Ceramic honeycomb structure |
US4080282A (en) * | 1976-07-12 | 1978-03-21 | Gulf Research & Development Company | Catalytic reactor and process for hydrogenating solid-containing carbonaceous materials in said reactor |
US4135018A (en) * | 1976-08-05 | 1979-01-16 | Corning Glass Works | Thermal shock resistant honeycomb structures |
US4328130A (en) * | 1980-10-22 | 1982-05-04 | Chevron Research Company | Shaped channeled catalyst |
DE3524775C1 (de) * | 1985-07-11 | 1986-09-04 | Daimler-Benz Ag, 7000 Stuttgart | In einem metallenen Gehaeuse angeordneter monolithischer Abgaskatalysator |
DE8605649U1 (de) * | 1986-03-01 | 1986-04-17 | Degussa Ag, 6000 Frankfurt | Vorrichtung zur Halterung von Monolithkatalysatoren |
JPS62297109A (ja) * | 1986-06-17 | 1987-12-24 | 日本碍子株式会社 | セラミツクハニカム構造体押出成形用ダイス |
US6029442A (en) * | 1996-12-18 | 2000-02-29 | Litex, Inc. | Method and apparatus for using free radicals to reduce pollutants in the exhaust gases from the combustion of fuel |
US6217832B1 (en) * | 1998-04-30 | 2001-04-17 | Catalytica, Inc. | Support structures for a catalyst |
-
2001
- 2001-03-13 US US09/804,944 patent/US7182924B2/en not_active Expired - Fee Related
-
2002
- 2002-03-05 WO PCT/US2002/006725 patent/WO2002072253A1/fr not_active Application Discontinuation
Patent Citations (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4195064A (en) * | 1978-08-15 | 1980-03-25 | Monsanto Company | Unitized catalytic reactor construction |
US4743578A (en) * | 1985-11-13 | 1988-05-10 | Imperial Chemical Industries Plc | Ceramic structures |
US5108716A (en) * | 1987-06-30 | 1992-04-28 | Nissan Motor Company, Inc. | Catalytic converter |
US6019951A (en) * | 1992-11-04 | 2000-02-01 | Technische Universiteit Delft | Catalytic reactor |
US5527631A (en) * | 1994-02-18 | 1996-06-18 | Westinghouse Electric Corporation | Hydrocarbon reforming catalyst material and configuration of the same |
WO1996033017A1 (fr) * | 1995-04-19 | 1996-10-24 | Technische Universiteit Delft | Procede de fabrication d'empilements de catalyseurs |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP3785795A4 (fr) * | 2018-07-13 | 2021-05-12 | Mitsubishi Heavy Industries Engineering, Ltd. | Réacteur catalytique |
US11413599B2 (en) | 2018-07-13 | 2022-08-16 | Mitsubishi Heavy Industries Engineering, Ltd. | Catalytic reactor |
Also Published As
Publication number | Publication date |
---|---|
US7182924B2 (en) | 2007-02-27 |
US20020131920A1 (en) | 2002-09-19 |
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